Unprecedented Relay Catalysis of Curved Fe1–N4 Single-Atom Site for Remarkably Efficient 1O2 Generation

催化作用 光化学 Atom(片上系统) 选择性 电子转移 双功能 化学 计算机科学 生物化学 嵌入式系统
作者
Man Yang,Keying Wu,Shaodong Sun,Jianglin Duan,Xin Liu,Jie Cui,Shuhua Liang,Yujing Ren
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:13 (1): 681-691 被引量:35
标识
DOI:10.1021/acscatal.2c05409
摘要

The design of catalysts and catalytic processes for high efficiency and selectivity of important singlet oxygen (1O2) active species generation in oxidation reactions is still challenging, especially utilizing abundant and environmental O2 without photoelectric field or extra thermal condition. Herein, a curved Fe1–N4 single-atom site is developed by incorporating isolated Fe single atom into nanodiamond with high-curvature surface. It leads to an unprecedented relay catalysis route, in which the activation of O2 is coupled with peroxymonosulfate (PMS) activation, to efficiently generate 1O2 species. In detail, PMS is first activated on the curved Fe1–N4 site with electron donation to Fe single atom, accompanied by 1/2 equiv of 1O2 production. More importantly, due to the compressive strain of the curved Fe1–N4 site with a higher energy level of Fe 3dz2 orbital, the curved Fe1–N4 site with electron charge acquisition can directly transfer electron to O2 molecule and consequently trigger the generation of additional 1 equiv of 1O2. Taking advantage of this tandem process, remarkable efficiency and near 100% selectivity of 1O2 generation are achieved, which leads to an ultrahigh metal catalytic efficiency of 0.77 min–1 for tetracycline oxidative degradation and an outstanding catalytic performance for benzene alcohol selective oxidation. This work, on the one hand, opens up an efficient way to generate 1O2 by O2 activation in peroxide-based catalytic oxidations, and on the other hand, develops a bifunctional Fe1–N4 single-atom site with rapid electron gain and loss ability, which sheds light on further improving catalytic performance in single-atom catalysts via relay catalysis mechanism.
最长约 10秒,即可获得该文献文件

科研通智能强力驱动
Strongly Powered by AbleSci AI
更新
PDF的下载单位、IP信息已删除 (2025-6-4)

科研通是完全免费的文献互助平台,具备全网最快的应助速度,最高的求助完成率。 对每一个文献求助,科研通都将尽心尽力,给求助人一个满意的交代。
实时播报
书虫发布了新的文献求助10
3秒前
4秒前
郭阳发布了新的文献求助10
4秒前
4秒前
7秒前
8秒前
醉熏的鑫完成签到,获得积分10
8秒前
李蕤蕤完成签到,获得积分10
9秒前
小唐尼发布了新的文献求助30
9秒前
10秒前
11秒前
Huang_being发布了新的文献求助10
12秒前
shawn发布了新的文献求助10
12秒前
12秒前
FashionBoy应助dara采纳,获得10
13秒前
着急的大米完成签到,获得积分20
14秒前
orixero应助hello采纳,获得10
14秒前
星辰大海应助顺利煎蛋采纳,获得10
15秒前
15秒前
17秒前
量子星尘发布了新的文献求助10
18秒前
18秒前
GGBOND发布了新的文献求助10
18秒前
19秒前
wu发布了新的文献求助10
19秒前
纳米酶催化完成签到,获得积分10
20秒前
pppp发布了新的文献求助10
21秒前
桐桐应助林宝雯采纳,获得10
21秒前
程程发布了新的文献求助10
23秒前
完美世界应助着急的大米采纳,获得10
23秒前
23秒前
23秒前
bkagyin应助冰琪采纳,获得10
23秒前
万能图书馆应助anna采纳,获得10
25秒前
28秒前
28秒前
dara完成签到,获得积分10
28秒前
hello完成签到,获得积分10
28秒前
29秒前
30秒前
高分求助中
A new approach to the extrapolation of accelerated life test data 1000
ACSM’s Guidelines for Exercise Testing and Prescription, 12th edition 500
‘Unruly’ Children: Historical Fieldnotes and Learning Morality in a Taiwan Village (New Departures in Anthropology) 400
Indomethacinのヒトにおける経皮吸収 400
Phylogenetic study of the order Polydesmida (Myriapoda: Diplopoda) 370
基于可调谐半导体激光吸收光谱技术泄漏气体检测系统的研究 350
Robot-supported joining of reinforcement textiles with one-sided sewing heads 320
热门求助领域 (近24小时)
化学 材料科学 医学 生物 工程类 有机化学 生物化学 物理 内科学 纳米技术 计算机科学 化学工程 复合材料 遗传学 基因 物理化学 催化作用 冶金 细胞生物学 免疫学
热门帖子
关注 科研通微信公众号,转发送积分 3989115
求助须知:如何正确求助?哪些是违规求助? 3531367
关于积分的说明 11253688
捐赠科研通 3269986
什么是DOI,文献DOI怎么找? 1804868
邀请新用户注册赠送积分活动 882078
科研通“疑难数据库(出版商)”最低求助积分说明 809105